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K2S2O8强化g-C3N4薄膜电极光电催化降解Cu(CN)32-并同步回收Cu
摘要点击 135  全文点击 41  投稿时间:2017-06-14  修订日期:2017-08-08
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中文关键词  铜氰络合物  光电催化氧化  石墨相氮化碳  过硫酸盐  非自由基氧化
英文关键词  cyanide and copper complex  photoelectrocatalytic  g-C3N4  peroxydisulfate  non-radical oxidation
作者单位E-mail
党聪哲 河北工业大学土木与交通学院, 天津 300401;中国科学院生态环境研究中心环境水质学国家重点实验室, 北京 100085 dangxiaozhe@sina.cn 
李一兵 河北工业大学土木与交通学院, 天津 300401 lybhebut@sina.com 
王彦斌 中国科学院生态环境研究中心环境水质学国家重点实验室, 北京 100085  
赵旭 中国科学院生态环境研究中心环境水质学国家重点实验室, 北京 100085 zhaoxu@rcees.ac.cn 
中文摘要
      采用高温液相生长法制得g-C3N4薄膜电极并作为光阳极,以石墨毡作为阴极,建立了光电催化系统.通过对比光电催化体系、K2S2O8体系以及外加K2S2O8到光电催化体系,发现在光电催化系统下外加K2S2O8可以有效地提高光电催化降解Cu(CN)32-的效率,并实现了Cu在阴极上的有效回收.探究了K2S2O8投加量对CN-降解率和Cu回收率的影响,发现当K2S2O8浓度为1 mmol·L-1,偏压为1.0 V时,CN-的去除率和Cu回收率分别达到86.23%和82.11%.通过SEM、EDS和XPS分析阴阳极表面形貌,发现部分Cu+被氧化以CuO的形式存在于沉淀和阳极表面,大部分铜离子通过电化学还原作用以单质铜的形式沉积于阴极表面,铜离子有效地从体系中去除.电子顺磁共振及淬灭实验分析表明,CN-的氧化去除是硫酸根自由基(SO4·-)氧化和非自由基氧化共同作用.
英文摘要
      Oxidation of Cu-cyanides by a photoelectrocatalytic method was enhanced by adding peroxydisulfate (PS). In the photoelectrocatalytic system (PEC), graphitic carbon nitride (g-C3N4) thin films prepared by a liquid-based reaction and graphitic carbon felt (GCF) were used as the photoanode and cathode, respectively. First, various processes, including PEC, PS oxidation, and PEC with PS addition (PEC/PS), were compared for Cu-cyanide removal. The addition of PS improved greatly the photoelectrocatalytic efficiency for the oxidation of CN- and the recovery of Cu on the cathode. The effect of the amount of K2S2O8 was investigated in detail. The removal efficiency of CN- and Cu recovery can reach up to 86.23% and 82.11%, respectively, with 1 mmol·L-1 K2S2O8 at 1.0 V bias potential. Combined with the SEM, EDS, and XPS analysis of the electrode surface, it was concluded that the free Cu+ was oxidized and existed in the precipitation and photoanode in the form of CuO. Conversely, the liberated Cu+/Cu2+ ions were electrochemically reduced to elemental Cu on the surface of the graphitic carbon felt cathode. As a result, metal Cu was recovered from the wastewater of the copper cyanide complexes. Electron spin resonance and radical quenching experiment analysis showed that the oxidation of CN- is assigned to sulfate radical oxidation and non-radical oxidation processes.

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